Extensive radioactive characterization of a phosphogypsum stack in SW Spain: 226Ra, 238U, 210po concentrations and 222Rn exhalation rate

Phosphogypsum (PG) is a by-product of the phosphate fertilizer industries that contains relatively high concentrations of uranium series radionuclides. The US-EPA regulates the agriculture use of PG, attending to its Ra-226 content and to the Rn-222 exhalation rate from inactive stacks. Measurements of Rn-222 exhalation rates in PG stacks typically show a large and still poorly understood spatial and temporal variability, and the published data are scarce. This work studies an inactive PG stack in SW Spain of about 0.5 km(2) from where PG can be extracted for agriculture uses, and an agriculture soil 75 km apart, being representative of the farms to be amended with PG. Activity concentrations of Ra-226, U-231 and Po-210 have been measured in 30 PG samples (0-90cm horizon) allowing for the construction of maps with spatial distributions in the PG stack and for the characterization of the associated PG inputs to agriculture soils. Averaged Ra-226 concentrations for the stack were 730 +/- 60 Bq kg(-1) (d.w.), over the US-EPA limit of 370 Bq kg(-1). Rn-222 exhalation rate has been measured by the charcoal canister method in 49 sampling points with 3 canisters per sampling point. Values in PG stack were under the US-EPA limit of 2600 Bq m(-2) h(-1), but they were one order of magnitude higher than those found in the agriculture soil. Variability in radon emissions has been studied at different spatial scales. Radon exhalation rates were correlated with Ra-226 concentrations and daily potential evapotranspiration (ETo). They increased with ETo in agriculture soils, but showed an opposite behaviour in the PG stack. (C) 2008 Elsevier B.V. All rights reserved.